Exciton Manifolds in Highly Ambipolar Doped WS2.

The disentanglement of single and many particle properties in 2D semiconductors and their dependencies on high carrier concentration is challenging to experimentally study by pure optical means. We establish an electrolyte gated WS2 monolayer field-effect structure capable of shifting the Fermi level from the valence into the conduction band that is suitable to optically trace exciton binding as well as the single-particle band gap energies in the weakly doped regime. Combined spectroscopic imaging ellipsometry and photoluminescence spectroscopies spanning large n- and p-type doping with charge carrier densities up to 1014 cm-2 enable to study screening phenomena and doping dependent evolution of the rich exciton manifold whose origin is controversially discussed in literature. We show that the two most prominent emission bands in photoluminescence experiments are due to the recombination of spin-forbidden and momentum-forbidden charge neutral excitons activated by phonons. The observed interband transitions are redshifted and drastically weakened under electron or hole doping. This field-effect platform is not only suitable for studying exciton manifold but is also suitable for combined optical and transport measurements on degenerately doped atomically thin quantum materials at cryogenic temperatures.

Low power all optical switching and implementation of universal logic gates using micro-bubbles in semiconductor nanocrystal solutions.

We describe optical switching in solutions of semiconductor nanocrystals illuminated by a 404 nm continuous wave laser source, driven by the formation of a micro-bubble of solvent vapor in the solution. Low boiling solvents such as hexane show an oscillatory modulation of transmitted light intensity (period ∼4 s) while solvents with intermediate boiling points such as toluene give a stable switching response. An on/off ratio of 83% is observed in the transmitted pump beam. Using this, a pump beam (404 nm, 80 mW continuous wave) was shown to reversibly switch the state of a probe laser (630 nm, 5 mW continuous wave). This switch thus serves as an optical analog of an electronic transistor and demonstrates the potential for all optical switching of low power light beams. Further, all optical universal logic gates, NAND and NOR, were also demonstrated using the micro-bubble switch.

Reconfiguring crystal and electronic structures of MoS2 by substitutional doping.

Doping of traditional semiconductors has enabled technological applications in modern electronics by tailoring their chemical, optical and electronic properties. However, substitutional doping in two-dimensional semiconductors is at a comparatively early stage, and the resultant effects are less explored. In this work, we report unusual effects of degenerate doping with Nb on structural, electronic and optical characteristics of MoS2 crystals. The doping readily induces a structural transformation from naturally occurring 2H stacking to 3R stacking. Electronically, a strong interaction of the Nb impurity states with the host valence bands drastically and nonlinearly modifies the electronic band structure with the valence band maximum of multilayer MoS2 at the Γ point pushed upward by hybridization with the Nb states. When thinned down to monolayers, in stark contrast, such significant nonlinear effect vanishes, instead resulting in strong and broadband photoluminescence via the formation of exciton complexes tightly bound to neutral acceptors.

Synthesis and spectroscopic characterization of alkali-metal intercalated ZrSe2.

We report on the synthesis and spectroscopic characterization of alkali metal intercalated ZrSe2 single crystals. ZrSe2 is produced by chemical vapour transport and then Li is intercalated. Intercalation is performed from the liquid phase (via butyllithium) and from the vapour phase. Raman spectroscopy of intercalated ZrSe2 reveals phonon energy shifts of the Raman active A1g and Eg phonon modes, the disappearance of two-phonon modes and new low wavenumber Raman modes. Angle-resolved photoemission spectroscopy is used to perform a mapping of the Fermi surface revealing an electron concentration of 4.7 × 1014 cm-2. We also perform vapour phase intercalation of K and Cs into ZrSe2 and observe similar changes in the Raman modes as for the Li case.

Angle of incidence averaging in reflectance measurements with optical microscopes for studying layered two-dimensional materials.

Reflectance spectrum measured using an optical microscope with a large numerical aperture objective lens is shown to get modified. The change is most prominent when there are optical interference related features in the spectrum. This modification is shown to arise primarily due to the wide range of angles of incidence involved in the measurement and a simple formulation is provided to correct for this in simulations. The importance of such analysis is brought out through a reflectance contrast spectroscopy based study for identifying mono-layer and bi-layer graphene and MoS2.